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https://doi.org/10.1007/s10800-018-1268-1
RESEARCH ARTICLE
Abstract
In this work, a screen-printed carbon paste electrode (SPCE) combined with multi-walled carbon nanotubes (MCNT) and
graphene (GP) in different mixing ratios was fabricated. Electrode materials were characterized by scanning electron micros-
copy as well as Raman spectroscopy and their performance as electrochemical sensors was evaluated by cyclic voltammetry.
Results showed that SPCEs composited with 1 w% MCNT and 1 w% graphene achieved the most promising sensing perfor-
mance for K4FeCN6 with a sensitivity of 0.0054 µA µM−1 and limit of detection (LOD) (3S/N) at 3.1 µM. The so-prepared
electrode was then employed to detect H2O2 and nicotinamide adenine dinucleotide (NAD+/NADH) achieving sensitivity
and LOD of 0.0027 µA µM−1 and 7.1 µM for H 2O2, and 0.0075 µA µM−1 and 3.6 µM for NADH, respectively. Therefore, it
was found that the addition of MCNT and graphene to commercial carbon paste for screen printable electrochemical sensor
is feasible for fabrication of sensing electrodes for electrochemical detection.
Graphical abstract
Keywords Screen-printed carbon paste electrode (SPCE) · Multi-walled carbon nanotube (MCNT) · Graphene (GP) ·
Electrochemical detection
1 Introduction
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Journal of Applied Electrochemistry
addition, they can be modified conveniently with sensitive with proper quantity to the carbon paste to fabricate screen-
membranes [8, 9], redox mediators, [10, 11] or enzymes printed electrodes. To do this, MCNT was added to the car-
[12, 13] to enhance specificity and sensitivity in detection bon paste to determine its optimum amount that achieved
systems. Moreover, their low cost and, thus, disposability satisfactory electrical conductivity at the lowest capacitive
make time-consuming cleaning processes for reuse obsolete. current. Following this, a small amount of GP was added to
One variety of SPEs used to detect analytes in sam- accelerate the charge transfer at the electrode surface. Over-
ples is carbon paste electrodes (CPE) [14–16]. Recently, all, the developed electrode provides clear faradaic currents
some researchers, including our group in this work, have for each analyte compared to its background current due to
attempted to increase the sensitivity and the limit of detec- its decreased capacitive current [30] which is beneficial for
tion (LOD) of CPEs by introducing conductive materials detection of analytes at ultratrace level.
in the carbon paste to fabricate as SPEs instead of using
sensitive membranes, redox mediators, or enzymes to avoid
inconstant properties and fouling of electrode surface. For 2 Experimental
instance, carbon paste can be easily mixed with graphene
powder and printed on plastic sheets to obtain screen-printed 2.1 Materials and methods
graphene electrode (SPGE) as was previously reported by us
and other groups [17–20]. Carbon rods (1/4″ diameter, Electron Microscopy Science)
Nowadays, graphene is one of the most frequently used were purchased from Becthai Company. Carbon paste and
carbon nanomaterials due to its high electrical conductiv- silver/silver chloride paste were bought from Gwent Com-
ity and large surface area compared to carbon nanotubes pany, UK. Insulating ink was purchased from Chaiyaboon
and graphite [21, 22]. Although graphene can be utilized to Brother Company, Pathumthani, Thailand. MCNT was
improve electrical conductivity of composite materials, it obtained from Chiangmai University, Thailand. Sodium
also causes a very high capacitive current of SPEs (> 1 µA). polystyrene sulfonate (PSS), K4FeCN6, β-nicotinamide ade-
This limits the applicability of graphene-based electrodes for nine dinucleotide, reduced dipotassium salt (NAD+/NADH),
monitoring analytes at ultratrace amount and with faradaic H2O2, NaH2PO4, and Na2HPO4 were purchased from Sigma
current to less than 1 µA. Previous reports [17–20] showed Aldrich. All chemicals were analytical grade and were used
that electrolyte solutions, measured using graphene-based without purification. Deionized water (18 MΩ∙cm) was used
electrodes, showed a very high capacitive current. This to prepare stock solutions. A MK Mini printer (Minami,
resulted in a significant decrease of faradaic current of the Japan) was employed to fabricate SPEs. Electrochemical
redox species. Therefore, analytes at ultratrace level could sensing experiments were performed using a µ-Autolab Type
not be detected if the capacitive current of the graphene- III, Metrohm, Switzerland. A Hitachi model S-4700 scan-
based electrodes is not properly reduced. ning electron microscope was employed to investigate the
In this work, a new sensing electrode was fabricated by surface morphology of each SPE. Additionally, Raman spec-
mixing carbon paste with quantities of MCNT and oxide- troscopy (NT-MDT model Ntegra spectra) was performed
free graphene to increase the electrical conductivity and to to characterize the electrodes.
decrease the peak potential of analytes. K 4FeCN6, H2O2 and
NADH (dissolved in 0.1 M pH 7 phosphate buffer solution) 2.2 Preparation of printing pastes and electrodes
were used to test the efficiency of the developed electrodes
and compare them with SPGE performance reported in our Graphene was prepared by electrolytic exfoliation. For this,
previous work. MCNT was chosen to be blended with the two carbon rods were immersed in a 3% (w/w) sodium poly-
graphene containing carbon paste, due to its excellent elec- styrene sulfonate (PSS) solution. A potential of 8 V was then
trical conductivity, large surface area, and chemical stability applied between them for 15 h leading to exfoliation of gra-
[23–25]. Furthermore, the excellent electron transfer ability phene sheets from the graphite. PSS stabilizes the dispersion
of MCNT plays an important role for electrochemical detec- and prevents restacking of graphene sheets. The graphene/
tion as confirmed by many other research works [26–29]. PSS dispersion was filtered with filter paper and washed
This article demonstrates the promising ways to utilize with ethanol and DI water several times. The collected sol-
both MCNT and graphene in the fabrication of sensing elec- ids were dried at 100 °C for 15 h and stored in a desiccator.
trodes which offer high electrical conductivity and which Figure 1 shows SEM micrographs of MCNT (Fig. 1a) and
can also detect analytes with higher sensitivity, lower LOD, oxide-free graphene (Fig. 1b) which were blended with the
and lower peak potential than SPGE. Even though, MCNT carbon paste for the fabrication of sensing electrode shown
and GP have both been widely applied as electrochemical in Fig. 2. As can be seen, MCNT features a fibrous structure
sensing materials, there is, to the best of our knowledge, no with variation of outer diameter sizes from 10 to 20 nm. The
work that explores the combined addition of MCNT and GP oxide-free graphene exhibits a two-dimensional structure
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Fig. 1 SEM micrographs of a
MCNT and b oxide-free gra-
phene synthesized by electro-
lytic exfoliation
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very high capacitive current (> 1 µA) makes it impossible The modified SPCE with the best detection performance was
to detect analyte quantities at ultratrace level. Thus, only selected to detect H2O2 and NADH in the next step. Addi-
SPCE with 1% (w/w) MCNT was employed for compositing tionally, the detection performance of our developed elec-
with graphene/PSS since it exhibits the lowest capacitive trode was compared to that of SPCE with 10% GP (SPGE) as
current compared to other modified SPCEs. In Fig. 4a, b, reported in our previous work [17] including other relevant
SPCE with 1% MCNT and 1% GP was employed to detect works.
K4FeCN6 to verify its performance. It was found that SPCE Figure 5 shows the surface morphologies of pure SPCE,
with 1% MCNT gave the detection sensitivity of K 4FeCN6 SPCE with 1% MCNT, and SPCE with 1% MCNT and
−1
at 0.0042 µA µM . 1% GP characterized by SEM to observe the filler disper-
Subsequently, SPCE with 1% MCNT was composited sion in the carbon paste. The surface of a pure SPCE in
with GP in different amounts (0.5%, 1%, 1.5%, and 2% Fig. 5a shows large roughness after treating at 60 °C for 1 h.
(w/w)). The electrodes were then used to detect K4FeCN6. However, the fibrous structure of MCNT of SPCE with 1%
Fig. 4 a Voltammograms of K 4FeCN6 between 10 and 1000 µM measured using SPCE with 1% MCNT and b the standard curve showing the
relation between the anodic current of K4FeCN6 and concentration range
Fig. 5 SEM micrographs of a a
blank SPCE, b SPCE with 1%
MCNT, and c SPCE with 1%
MCNT + 1% GP, respectively
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MCNT in Fig. 5b could not be observed in comparison to the dispersion of MCNT and GP in the carbon paste by
a pristine MCNT as shown in Fig. 1a because it was fully the raised intensity of the 2D band. For all of the elec-
covered with carbon paste. Overall, the surface morphology trodes, the D band appeared at Raman shift between 1305
of the electrode presents higher roughness due to agglomera- and 1310 cm−1, at 1577–1578 cm−1 for the G band and at
tion between MCNT particle and the carbon paste. Further- 2625–2630 cm−1 for the 2D band. However, a pure SPCE
more, MCNT also causes higher roughness of the electrode showed the highest intensity of D and G bands among
surface; thus, it should not be added to the carbon paste with all electrodes while its 2D band had the lowest intensity.
a greater amount than 1%. For SPCE with 1% MCNT and When SPCE contained 1% MCNT and 1% GP, the inten-
1% GP, MCNT and GP particles evidently do not appear sity of the 2D band was comparable to that of SPCE with
in the SEM micrograph displayed in Fig. 5c. However, its 1% MCNT and pure SPCE.
surface roughness is not as large as in SPCE samples with The results shown in Fig. 7 suggest that SPCE with
1% MCNT. This is probably due to presence of oxygen- 1% MCNT and 1% GP was the most promising elec-
containing functional groups on GP, which results in lower trode among all types due to its highest S/B ratio. As
roughness of composited ink. the results shown in Fig. 7, SPCE with 1% MCNT and
In addition, Raman spectra of pure SPCE, SPCE with 1% GP presents the greatest efficiency in detection of
1% MCNT, and SPCE with 1% MCNT and 1% GP were 1000 µM K4FeCN6. The reason for this is probably that
investigated and are displayed in Fig. 6. Results confirm GP has excellent electrical conductivity which will pro-
mote charge transfer at the electrode surface. Moreover,
only 1% MCNT and 1% GP can be well dispersed in the
carbon paste, which affects the highest value of S/B (20.4)
compared to other mixing ratios. In summary, SPCE with
1% MCNT and 0.5% GP is not sufficiently efficient for
electrochemical detection. Meanwhile, both 1.5% and 2%
GP may be an excessive amount, which causes the large
agglomeration of fillers in the carbon paste and higher
peak potential of analytes. Therefore, SPCE with 1%
MCNT and 1% GP (from here on denoted SPCE/CNT1%/
G1%) is the most promising electrode and was also applied
for detection of H
2O2 and NADH in the following study to
verify its detection performance.
Fig. 7 a Comparing the anodic current signal (S) of 1000 µM K4FeCN6 measured by SPCE with 1% MCNT after mixing GP at 0.5%, 1%, 1.5%,
and 2% (w/w) and b the ratio of S/B of each electrode
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Fig. 11 Voltammograms of a 1000 µM K4FeCN6, b 1000 µM H2O2, and c 1000 µM NADH measured by different scan rates (20–250 mV/s), as
well as d the standard curve plotted between the anodic current (µA) of each analyte and the scan r ate1/2 (mV S−1)1/2
In addition, the developed electrode promoted the elec- by electrode modification to increase the selectivity to ana-
tron transfer ability of analytes. This result is affirmed by lytes of interest.
the peak potential decreased of K4FeCN6 (0.29–0.31 V),
H2O2 (0.8–0.85 V), and NADH (0.45–0.5 V) compared 3.5 Repeatability and reproducibility study
to inkjet-printed GP-PEDOT:PSS electrode employed to
detect K4FeCN6 (0.3–0.42 V), H2O2 (0.8–1.0 V), and NADH The repeatability of SPCE/CNT1%/G1% was evaluated by
(0.6–0.65 V) as studied from another previous work of our recording cyclic voltammogram for 10 successive cycles.
group [34]. From the results, our electrode still reserved the stability
Overall, K4FeCN6, H2O2, and NADH are common ana- towards the oxidation of each analyte up to 10 successive
lytes that can be detected using our developed electrode. The cycles with relative standard deviation (RSD, n = 10), such
results suggest that this electrode could be also employed as 5.25% for K4FeCN6, 7.26% for H2O2, and 3.70% for
to monitor other analytes. However, the performance of NADH. Moreover, the reproducibility for electrochemical
this developed electrode on the detection of real samples detection was estimated from 10 electrodes. It was found
will have to be further studied by sample pretreatment or that the developed electrode exhibited a good reproducibility
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Fig. 12 Voltammograms of a K4FeCN6, b H2O2, and c NADH measured using SPCE with 1% MCNT and 1% GP, and d their standard curve
plotted between the anodic current and concentration range between 10 and 1000 µM
(RSD, n = 10), namely 10.39% for K4FeCN6, 8.71% for only SPCE/CNT1%/G1% is greatly useful to increase sensi-
H2O2, and 3.39% for NADH, respectively. tivity and to decrease LOD (3S/N) of analyte detection.
Most importantly, the developed electrode is able to detect
K4FeCN6, H2O2, and NADH with lower peak potential and
4 Conclusions lower linear range (10–1000 µM). Therefore, our work is a
beneficial guidance to apply the advantages of both MCNT
In this work, SPCE/CNT1%/G1% exhibited a very good per- and GP materials in the fabrication of screen-printed elec-
formance towards electrochemical detection for K
4FeCN6, trode for electrochemical detection.
AD+/NADH among all electrodes. Interestingly,
H2O2, and N
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Table 1 Data from comparing the performance of SPCE with 1% MCNT and 1% GP, and the previous works
Acknowledgements The authors are grateful for the research grant for sensor based on an electropolymerized metal organic framework.
project (P1851485) from National Electronics and Computer Technol- Toxins 7:3540–3553. https://doi.org/10.3390/toxins7093540
ogy Center (NECTEC), National Science and Technology Develop- 8. Shoukry AF, Badawy SS, Issa YM (1987) Diphenhydramine-sen-
ment Agency (NSTDA), and from Thailand Research Fund for TRF sitive membrane electrodes based on poly(vinylchloride) matrices
Research Team Promotion Grant (RTA6180004). and their use in drug analysis. J Electroanal Chem Interfacial Elec-
trochem 233:29–36. https: //doi.org/10.1016/0022-0728(87)85003
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Affiliations
1 2
Graphene and Printed Electronics Research Team (GPE), Opto‑Electrochemical Sensing Research Team (OEC),
National Electronics and Computer Technology Center National Electronics and Computer Technology Center
(NECTEC), 112 Thailand Science Park, Phahonyothin Road, (NECTEC), 112 Thailand Science Park, Phahonyothin Road,
Khlong Neung, Khlongluang, Pathumthani 12120, Thailand Khlong Neung, Khlongluang, Pathumthani 12120, Thailand
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